Bioinspired molecular clusters for water oxidation

Chen, Qifa; Guo, Yu‐Hua; Yu, Yi-Han; Zhang, Ming‐Tian

doi:10.1016/j.ccr.2021.214164

Cited by 33 publications

(23 citation statements)

References 158 publications

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“…It is hence of great significance to develop efficient and stable water oxidation catalysts (WOCs). 5–8 For WOCs based on transition metal complexes, their multidentate organic ligand facilitates structure modification. To understand the catalytic mechanism, investigations have been conducted to establish a relationship between the structure and catalytic activity.…”

Section: Introductionmentioning

confidence: 99%

Electrocatalytic water oxidation by copper(ii) complexes with a pentadentate amine-pyridine ligand

Lin

Wang

Chen

et al. 2022

Sustainable Energy Fuels

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Section: Introductionmentioning

confidence: 99%

Electrocatalytic water oxidation by copper(ii) complexes with a pentadentate amine-pyridine ligand

Lin

Wang

Chen

et al. 2022

Sustainable Energy Fuels

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“…To facilitate the understanding of the structure and properties of the OEC, as well as for developing efficient water-splitting catalysts, many research groups, during the last three decades, have attempted to synthesize the OEC ( Wieghardt, 1989 ; Limburg et al, 1999 ; Mukhopadhyay et al, 2004 ; Mullins and Pecoraro, 2008 ; Dismukes et al, 2009 ; Gerey et al, 2016 ; Zhang and Sun, 2019b ; Li et al, 2020b ; Chen et al, 2021 ; Ezhov et al, 2021 ). It is a great challenge and a long-standing issue for chemists to synthesize the OEC in the laboratory ( Zhang, 2015 ; Li et al, 2020b ).…”

Section: Mimicking the Oecmentioning

confidence: 99%

Mimicking the Oxygen-Evolving Center in Photosynthesis

Chen

Yao

et al. 2022

Front. Plant Sci.

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The oxygen-evolving center (OEC) in photosystem II (PSII) of oxygenic photosynthetic organisms is a unique heterometallic-oxide Mn4CaO5-cluster that catalyzes water splitting into electrons, protons, and molecular oxygen through a five-state cycle (Sn, n = 0 ~ 4). It serves as the blueprint for the developing of the man-made water-splitting catalysts to generate solar fuel in artificial photosynthesis. Understanding the structure–function relationship of this natural catalyst is a great challenge and a long-standing issue, which is severely restricted by the lack of a precise chemical model for this heterometallic-oxide cluster. However, it is a great challenge for chemists to precisely mimic the OEC in a laboratory. Recently, significant advances have been achieved and a series of artificial Mn4XO4-clusters (X = Ca/Y/Gd) have been reported, which closely mimic both the geometric structure and the electronic structure, as well as the redox property of the OEC. These new advances provide a structurally well-defined molecular platform to study the structure–function relationship of the OEC and shed new light on the design of efficient catalysts for the water-splitting reaction in artificial photosynthesis.

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“…Solar-driven water splitting to produce hydrogen fuel is an attractive strategy for coping with the future energy crisis. − In trying to achieve this goal, scientists are learning the secrets of nature’s photosynthesis , as inspiration for developing artificial catalytic systems. Water oxidation is a bottleneck in the development of artificial photosynthetic processes, − as shown by previous studies on molecular water oxidation catalysts based on Ru-, − Ir-, , Mn-, , Co-, − Ni, − and Fe − complexes, because the main obstacle is our limited knowledge on how to regulate the O–O bond formation. In contrast, the mechanism of dioxygen activation and the associated O–O bond cleavage is well documented, especially for copper enzymes. − Inspired by this Cu/O 2 chemistry, Mayer and his co-workers reported the first homogeneous copper catalyst, (bpy)Cu(OH) 2 , for electrocatalyzed water oxidation in an alkaline solution .…”

Section: Introductionmentioning

confidence: 99%

Bioinspired Trinuclear Copper Catalyst for Water Oxidation with a Turnover Frequency up to 20000 s^–1

et al. 2021

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Solar-powered water splitting is a dream reaction for constructing an artificial photosynthetic system for producing solar fuels. Natural photosystem II is a prototype template for research on artificial solar energy conversion by oxidizing water into molecular oxygen and supplying four electrons for fuel production. Although a range of synthetic molecular water oxidation catalysts have been developed, the understanding of O−O bond formation in this multielectron and multiproton catalytic process is limited, and thus water oxidation is still a big challenge. Herein, we report a trinuclear copper cluster that displays outstanding reactivity toward catalytic water oxidation inspired by multicopper oxidases (MCOs), which provides efficient catalytic four-electron reduction of O 2 to water. This synthetic mimic exhibits a turnover frequency of 20000 s −1 in sodium bicarbonate solution, which is about 150 and 15 times higher than that of the mononuclear Cu catalyst (F−N 2 O 2 Cu, 131.6 s −1 ) and binuclear Cu 2 complex (HappCu 2 , 1375 s −1 ), respectively. This work shows that the cooperation between multiple metals is an effective strategy to regulate the formation of O−O bond in water oxidation catalysis.

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Bioinspired molecular clusters for water oxidation

Cited by 33 publications

References 158 publications

Electrocatalytic water oxidation by copper(ii) complexes with a pentadentate amine-pyridine ligand

Electrocatalytic water oxidation by copper(ii) complexes with a pentadentate amine-pyridine ligand

Mimicking the Oxygen-Evolving Center in Photosynthesis

Bioinspired Trinuclear Copper Catalyst for Water Oxidation with a Turnover Frequency up to 20000 s^–1

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Bioinspired molecular clusters for water oxidation

Cited by 33 publications

References 158 publications

Electrocatalytic water oxidation by copper(ii) complexes with a pentadentate amine-pyridine ligand

Electrocatalytic water oxidation by copper(ii) complexes with a pentadentate amine-pyridine ligand

Mimicking the Oxygen-Evolving Center in Photosynthesis

Bioinspired Trinuclear Copper Catalyst for Water Oxidation with a Turnover Frequency up to 20000 s–1

Contact Info

Product

Resources

About

Bioinspired Trinuclear Copper Catalyst for Water Oxidation with a Turnover Frequency up to 20000 s^–1